US7239072B2 - Fluorescent lamp and method of manufacturing - Google Patents

Fluorescent lamp and method of manufacturing Download PDF

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Publication number
US7239072B2
US7239072B2 US10/516,150 US51615004A US7239072B2 US 7239072 B2 US7239072 B2 US 7239072B2 US 51615004 A US51615004 A US 51615004A US 7239072 B2 US7239072 B2 US 7239072B2
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United States
Prior art keywords
discharge
lamp
translucent layer
low
pressure mercury
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Expired - Fee Related, expires
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US10/516,150
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English (en)
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US20050206320A1 (en
Inventor
Ingrid Jozef Maria Snijkers-Hendrickx
Henricus Albertus Maria Van Hal
Wilhelmus Cornelis Keur
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Koninklijke Philips NV
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Koninklijke Philips Electronics NV
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Assigned to KONINKLIJKE PHILIPS ELECTRONICS N.V. reassignment KONINKLIJKE PHILIPS ELECTRONICS N.V. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: KUER, WILHELMUS CORNELIS, SNIJKERS-HENDRICKX, INGRID JOZEF MARIA, VAN HAL, HENRICUS ALBERTUS MARIA
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J9/00—Apparatus or processes specially adapted for the manufacture, installation, removal, maintenance of electric discharge tubes, discharge lamps, or parts thereof; Recovery of material from discharge tubes or lamps
    • H01J9/24—Manufacture or joining of vessels, leading-in conductors or bases
    • H01J9/34—Joining base to vessel
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J61/00—Gas-discharge or vapour-discharge lamps
    • H01J61/02—Details
    • H01J61/24—Means for obtaining or maintaining the desired pressure within the vessel
    • H01J61/26—Means for absorbing or adsorbing gas, e.g. by gettering; Means for preventing blackening of the envelope
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J61/00—Gas-discharge or vapour-discharge lamps
    • H01J61/02—Details
    • H01J61/30—Vessels; Containers
    • H01J61/32—Special longitudinal shape, e.g. for advertising purposes
    • H01J61/327—"Compact"-lamps, i.e. lamps having a folded discharge path
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J61/00—Gas-discharge or vapour-discharge lamps
    • H01J61/02—Details
    • H01J61/30—Vessels; Containers
    • H01J61/35—Vessels; Containers provided with coatings on the walls thereof; Selection of materials for the coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
    • H01J61/00—Gas-discharge or vapour-discharge lamps
    • H01J61/70—Lamps with low-pressure unconstricted discharge having a cold pressure < 400 Torr
    • H01J61/72—Lamps with low-pressure unconstricted discharge having a cold pressure < 400 Torr having a main light-emitting filling of easily vaporisable metal vapour, e.g. mercury

Definitions

  • the invention relates to a low-pressure mercury-vapor discharge lamp comprising a light-transmitting discharge vessel, the discharge vessel enclosing, in a gastight manner, a discharge space provided with a filling of mercury and a rare gas, the discharge vessel comprising means for maintaining a discharge in the discharge space, while at least a portion of an inner wall of the discharge vessel is provided with a translucent layer.
  • the invention also relates to a compact fluorescent lamp.
  • the invention in addition, relates to a method of manufacturing a fluorescent lamp.
  • mercury constitutes the primary component for the (efficient) generation of ultraviolet (UV) light.
  • a luminescent layer comprising a luminescent material (for example, a fluorescent powder) may be present on an inner wall of the discharge vessel to convert UV to other wavelengths, for example, to UV-B and UV-A for tanning purposes (sun panel lamps) or to visible radiation for general illumination purposes.
  • Such discharge lamps are therefore also referred to as fluorescent lamps.
  • the discharge vessel of a low-pressure mercury-vapor discharge lamp is usually tubular and circular in cross-section and comprises both elongate and compact embodiments.
  • the tubular discharge vessel of so-called compact fluorescent lamps comprises a collection of relatively short straight parts having a relatively small diameter, which straight parts are connected together by means of bridge parts or arc-shaped parts.
  • Compact fluorescent lamps are usually provided with an (integrated) lamp cap.
  • a low-pressure mercury-vapor discharge lamp of the type described in the opening paragraph is known from WO-A 01/56350.
  • the translucent layer provided on an inner surface of the discharge vessel of the know low-pressure mercury-vapor discharge lamp comprises a borate or a phosphate of an alkaline-earth metal and/or of scandium, yttrium, or another rare earth metal.
  • the translucent layer in the known discharge lamp has a thickness of between 5 and 200 nm.
  • a drawback of the use of the known low-pressure mercury-vapor discharge lamp is that its lumen maintenance still is relatively poor due to said blackening. As a result, in addition, a relatively large amount of mercury is necessary for the known lamp in order to realize a sufficiently long service life. This is detrimental to the environment in the case of injudicious processing after the end of the service life.
  • a low-pressure mercury-vapor discharge lamp of the type described in the opening paragraph which has an improved lumen maintenance.
  • a low-pressure mercury-vapor discharge lamp of the kind mentioned in the opening paragraph is for this purpose characterized in that the translucent layer comprises an alkaline earth borate, and in that the thickness of the translucent layer is in a range from 1 to 50 ⁇ m.
  • a discharge vessel of a low-pressure mercury-vapor discharge lamp according to the invention with a translucent layer having the above composition and with a thickness in the range given above appears to be very well resistant to the action of the mercury and rare gas atmosphere which, in operation, prevails in the discharge vessel of the low-pressure mercury-vapor discharge lamp.
  • blackening due to interaction between mercury and the glass from which the discharge vessel is manufactured is reduced, resulting in an improved lumen maintenance.
  • a smaller quantity of mercury is withdrawn from the discharge, so that, in addition, a reduction of the mercury consumption of the discharge lamp is obtained and a smaller mercury dose will suffice in the manufacture of the low-pressure mercury-vapor discharge lamp.
  • Blackening caused by removal of mercury from the discharge occurs in straight parts as well as in arc-shaped parts of the low-pressure mercury-vapor discharge lamp.
  • blackening is reduced by providing the inner wall of the discharge vessel with a sufficiently adhering and sufficiently thick translucent layer.
  • the arc-shaped lamp parts of compact fluorescent lamps are more subject to blackening than the straight lamp parts.
  • the arc-shaped lamp parts are generally not bent until after the tubular discharge vessel has been provided with the translucent layer and, if necessary, a luminescent layer. In the bending operation, the thickness of the translucent layer in the arc-shaped lamp parts is reduced and the translucent layer is stretched, which may result in the formation of cracks in the translucent layer.
  • the translucent layer is made by flushing the discharge vessel with a solution of a mixture of suitable metal-organic compounds, for example yttrium acetate mixed with calcium, strontium, and/or barium acetate, and an acid diluted in water, for example boric acid, while the desired translucent layer is obtained after drying and sintering.
  • a mixture of suitable metal-organic compounds for example yttrium acetate mixed with calcium, strontium, and/or barium acetate
  • an acid diluted in water for example boric acid
  • the thickness of the translucent layer is limited to a few 100 nm.
  • a translucent layer can be made with a thickness which can be significantly larger than that of the translucent layer made from the salts in the known discharge lamp.
  • the term “nano-particles” in the description of the present invention denotes that particles with a particle size in the range from 0.1 to 1 ⁇ m.
  • the softening point of the calcium, strontium, and/or barium borate particulate material is low enough for the particles to fuse together during the bending process.
  • a dense translucent layer is obtained that, because of its large thickness, has not completely reacted with the subjacent wall of the discharge vessel.
  • a translucent layer according to the invention made from nano-particles of calcium, strontium, and/or barium borate showed a relatively high point of zero charge and a relatively low mercury consumption.
  • An additional advantage of producing the translucent layer from nano-particles of alkaline earth borates is that the size of the particles of alkaline earth borates is comparable to the wavelength of the UV light. This makes it possible to employ the translucent layer also as a reflector for UV light (the size of the particles is in the range from approximately 0.5 ⁇ m to approximately 0.6 ⁇ m).
  • the measure according to the invention is notably suitable for compact fluorescent lamps having arc-shaped lamp parts, wherein the discharge vessel is additionally surrounded by a light-transmitting envelope.
  • the temperature of the discharge vessel of such “covered” compact fluorescent lamps is comparatively high because the heat dissipation to the environment is reduced by the presence of the envelope. This unfavorable temperature balance adversely affects the lumen maintenance of the known discharge lamp due to an increased level of blackening.
  • the translucent layer in the low-pressure mercury-vapor discharge lamp in accordance with the invention further satisfies the requirements with respect to light and radiation transmissivity and can be easily provided as a homogeneous translucent layer on an inner wall of a discharge vessel of a low-pressure mercury-vapor discharge lamp.
  • Translucent layers as thick as 50 ⁇ m, can be made with the alkaline earth borate nano-particles.
  • Strontium borate nano-particles are particularly suitable for producing such thick layers.
  • Making the translucent layer thicker than approximately 50 ⁇ m would give rise to lumen losses in the low-pressure mercury-vapor discharge lamp.
  • the thickness of the translucent layer is in the range from 1 to 20 ⁇ m.
  • the translucent layer is a translucent layer with a thickness in the range from 10 to 20 ⁇ m.
  • a translucent layer thinner than approximately 10 ⁇ m could give rise to a complete reaction of the particulate calcium, strontium, and/or barium borate with the wall, in particular during bending of discharge vessels under factory conditions. The risk is higher in a production environment where the conditions cannot always be met as precisely as in laboratory experiments. It is observed that the particles in the translucent layer do not reach a temperature high enough for melting in the straight parts of the discharge vessels of compact fluorescent lamps, thus leading to diffuse scattering of light in the translucent layer. In the arc-shaped parts of the discharge vessel of compact fluorescent lamps, the particles in the translucent layer do reach a temperature high enough for melting, thus leading to a transparent layer.
  • the translucent layer further comprises scandium, yttrium, or a further rare earth metal. Such materials provide an extra protection against wall blackening.
  • yttrium oxide is known in the art as a protective layer.
  • a preferred embodiment of the low-pressure mercury-vapor discharge lamp according to the invention is characterized in that the discharge vessel is made from a glass comprising silicon dioxide and sodium oxide, with the glass composition comprising the following essential constituents, given in percentages by weight: SiO 2 : 60 to 80% and Na 2 O: 10 to 20% by weight.
  • the application of a translucent layer according to the invention in combination with the sodium-rich glass in accordance with the invention causes blackening to be substantially reduced in the straight parts as well as in the arc-shaped parts of the low-pressure mercury-vapor discharge lamp.
  • the glass composition preferably comprises the following constituents: SiO 2 : 70 to 75%, Na 2 O: 15 to 18% and K 2 O: 0.25 to 2% by weight.
  • the composition of such a sodium-rich glass is similar to that of ordinary window glass and it is comparatively cheap with respect to the glass used in the known discharge lamp.
  • the cost price of the raw materials for the sodium-rich glass as used in the discharge lamp in accordance with the invention is only approximately 50% of the cost price of the raw materials for the mixed alkali glass as used in the known discharge lamp.
  • the use of the translucent layer according to the invention yields a low-pressure mercury-vapor discharge lamp with a relatively low mercury consumption with soda-lime glass as the wall material of the discharge vessel.
  • a preferred embodiment of the low-pressure mercury-vapor discharge lamp according to the invention is characterized in that a side of the translucent layer facing the discharge space is provided with a layer of a luminescent material.
  • An advantage of the use of a translucent layer according to the invention in low-pressure mercury-vapor discharge lamps is that the luminescent layer comprising a luminescent material (for example, a fluorescent powder) adheres significantly better to such a translucent layer than to a translucent layer of the known low-pressure mercury-vapor discharge lamp. Said improved adhesion is obtained particularly in the arc-shaped parts of low-pressure mercury-vapor discharge lamps.
  • the invention further relates to a method of manufacturing a fluorescent lamp, wherein a light-transmitting discharge vessel is provided so as to enclose, in a gastight manner, a discharge space provided with a filling of mercury and a rare gas, wherein the discharge vessel is provided with means for maintaining a discharge in the discharge space, and wherein at least a portion of an inner wall of the discharge vessel is provided with a translucent layer, characterized in that alkaline earth borate particles are used to form the translucent layer, the size of the calcium, strontium, and/or barium borate particles being in a range from 0.1 to 1 ⁇ m.
  • FIG. 1A is a cross-sectional view of an embodiment of a compact fluorescent lamp comprising a low-pressure mercury-vapor discharge lamp according to the invention.
  • FIG. 1B is a cross-sectional view of a detail of the low-pressure mercury-vapor discharge lamp as shown in FIG. 1A .
  • FIG. 1 shows a compact fluorescent lamp comprising a low-pressure mercury-vapor discharge lamp.
  • the low-pressure mercury-vapor discharge lamp is provided with a radiation-transmitting discharge vessel 10 enclosing, in a gastight manner, a discharge space 11 having a volume of approximately 10 cm 3 .
  • the discharge vessel 10 is a glass tube which is at least substantially circular in cross-section and the (effective) internal diameter D of which is approximately 10 mm.
  • the tube is bent in the form of a so-called hook and, in this embodiment, it has a number of straight parts, two of which, referenced 31 , 33 , are shown in FIG. 1A .
  • the discharge vessel further comprises a number of arc-shaped parts, two of which, referenced 32 , 34 , are shown in FIG.
  • An inner wall 12 of the discharge vessel 10 is provided with a translucent layer 16 according to the invention and with a luminescent layer 17 . In an alternative embodiment, the luminescent layer has been omitted.
  • the discharge vessel 10 is supported by a housing 70 which also supports a lamp cap 71 provided with electrical and mechanical contacts 73 a , 73 b , which are known per se.
  • the discharge vessel 10 of the low-pressure mercury-vapor discharge lamp is surrounded by a light-transmitting envelope 60 which is attached to the lamp housing 70 .
  • the light-transmitting envelope 60 generally has a matt appearance.
  • FIG. 1B is a very diagrammatic cross-sectional view of a detail of the low-pressure mercury-vapor discharge lamp shown in FIG. 1A .
  • the discharge space 11 in the discharge vessel 10 does not only comprise mercury but also a rare gas, argon in this example.
  • Means for maintaining a discharge are constituted by an electrode pair 41 a (only one electrode is shown in FIG. 1B ) which is arranged in the discharge space 11 .
  • the electrode pair 41 a is a winding of tungsten coated with an electron-emissive material, here a mixture of barium oxide, calcium oxide, and strontium oxide.
  • Each electrode 41 a is supported by an (indented) end portion of the discharge vessel 10 (not shown in FIGS. 1A and 1B ).
  • Current supply conductors 50 a , 50 a ′ issue from the electrode pair 41 a through the end portions of the discharge vessel 10 to the exterior.
  • the current supply conductors 50 a , 50 a ′ are connected to an (electronic) power supply which is accommodated in the housing 70 and electrically connected to the electrical contacts 73 b at the lamp cap 71 (see FIG. 1A ).
  • the glass of the wall of the discharge vessel of the low-pressure mercury-vapor discharge lamp has a composition comprising silicon dioxide and sodium oxide as important constituents.
  • the discharge vessel is made from a so-called sodium-rich glass, for example a glass of the following composition: 70 to 74% SiO 2 , 16 to 18% Na 2 O, 0.5 to 1.3% K 2 O, 4 to 6% CaO, 2.5 to 3.5% MgO, 1 to 2% Al 2 O 3 , 0 to 0.6% Sb 2 O 3 , 0 to 0.15% Fe 2 O 3 , and 0 to 0.05% MnO by weight.
  • the so-called nano-particles of SrB 4 O 7 with a particle size in the range from approximately 0.1 to approximately 1 ⁇ m are used to manufacture the translucent layer 16 according to the invention.
  • Stoichiometric quantities of SrCO 3 and H 3 BO 3 are mixed and melted in a Pt crucible in air. After cooling down, the glass is crushed and milled with butyl acetate during two hours followed by 48 hours rolling with ZrO 2 balls.
  • the resulting amorphous particles of SrB 4 O 7 have an average particle size of 0.6 ⁇ m.
  • Tubular discharge vessels were provided with a coating. After this coating operation, the discharge vessels were first dried in air at a temperature of approximately 60° C. for 15 minutes.
  • the transparent coating is fixed in a shorter period of time at a higher temperature.
  • the thickness of the translucent layer 16 ranges from approximately 1 ⁇ m to approximately 50 ⁇ m, preferably from approximately 10 ⁇ m to approximately 20 ⁇ m.
  • nano-particles of BaB 4 O 7 or CaB 4 O 7 are used.
  • the discharge vessels were provided with a luminescent coating comprising three known phosphors, namely a green-luminescing material with terbium-activated cerium-magnesium aluminate, a blue-luminescing material with bivalent europium-activated barium-magnesium aluminate, and a red-luminescing material with trivalent europium-activated yttrium oxide.
  • the discharge vessels were bent in the known “hook” shape having straight parts and arcuate parts. A number of said discharge vessels were subsequently assembled into low-pressure mercury-vapor discharge lamps in the customary manner.
  • the lumen maintenance after 1,000 and 2,000 hours was measured for low-pressure mercury-vapor discharge lamps comprising the known discharge vessel made from a sodium-rich glass provided with a translucent layer ( 16 ) in accordance with the invention with a thickness of approximately 15 ⁇ m, which translucent layer is made from SrB 4 O 7 nano-particles with an average size of 0.6 ⁇ m in accordance with the invention.
  • the result of this measurement is shown in Table I.
  • the lumen maintenance is standardized in a customary manner with respect to the value after 100 burning hours of the discharge lamp.
  • Lumen Maintenance of compact low-pressure mercury-vapor discharge lamps comprising the known discharge vessel made from a sodium-rich glass provided with a translucent layer in accordance with the invention.
  • Lumen Maintenance (%) 230 mm (11 W) 405 mm (20 W) 1000 hrs 2000 hrs 1000 hrs 2000 hrs with translucent 94 90 97 94 envelope layer based on SrB 4 O 7 nano- particles no 87 77 83 72 translucent layer without translucent 97 93 95 92 envelope layer based on SrB 4 O 7 nano- particles no 92 89 91 85 translucent layer
  • Table I shows that after 1,000 and 2,000 hours the lumen maintenance of discharge lamps comprising the known discharge vessel and provided with the translucent layer according to the invention is substantially improved. The largest improvement is obtained in discharge lamps provided with a light-transmitting envelope.
  • a translucent layer according to the invention in combination with the sodium-rich glass in accordance with the invention causes blackening to be substantially reduced in the straight parts as well as in the arc-shaped parts of the low-pressure mercury-vapor discharge lamp.
  • Wall blackening due to interaction between mercury and the glass of the discharge vessel is reduced, resulting in an improved lumen maintenance.
  • a smaller quantity of mercury is withdrawn from the discharge during the service life of the low-pressure mercury-vapor discharge lamp, so that a reduction of the mercury consumption of the discharge lamp is obtained and a smaller mercury dose suffices in the manufacture of the low-pressure mercury-vapor discharge lamp.

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Vessels And Coating Films For Discharge Lamps (AREA)
US10/516,150 2002-06-05 2003-05-27 Fluorescent lamp and method of manufacturing Expired - Fee Related US7239072B2 (en)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
EP02077200 2002-06-05
EP02077200.0 2002-06-05
EP02077200 2002-06-05
PCT/IB2003/002399 WO2003105184A2 (fr) 2002-06-05 2003-05-27 Lampe fluorescente et procede de fabrication

Publications (2)

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US20050206320A1 US20050206320A1 (en) 2005-09-22
US7239072B2 true US7239072B2 (en) 2007-07-03

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US (1) US7239072B2 (fr)
EP (1) EP1514293A2 (fr)
JP (1) JP2005529461A (fr)
CN (1) CN100377287C (fr)
AU (1) AU2003241091A1 (fr)
WO (1) WO2003105184A2 (fr)

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US20050182461A1 (en) * 2003-12-09 2005-08-18 Medx Health Corp. Shape-adaptable and spectral-selective distributed light sources using passive host medium
US20060271132A1 (en) * 2003-05-24 2006-11-30 Ledeep Llc Skin tanning and light therapy system and method
US20080039907A1 (en) * 2004-04-12 2008-02-14 Ledeep, Llc Phototherapy Systems and Methods
US20090230837A1 (en) * 2008-03-13 2009-09-17 General Electric Company Fluorescent lamps having desirable mercury consumption and lumen run-up times
US7591279B2 (en) 2001-08-24 2009-09-22 Cummins Filtration Ip Inc. Controlled release of additives in fluid systems
US7921853B2 (en) 2004-03-09 2011-04-12 Ledeep Llc Phototherapy method for treating psoriasis
US8425772B2 (en) 2006-12-12 2013-04-23 Cummins Filtration Ip, Inc. Filtration device with releasable additive

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EP1514295A1 (fr) * 2002-06-04 2005-03-16 Koninklijke Philips Electronics N.V. Lampe a decharge a vapeur de mercure et a basse pression et lampe fluorescente compacte
EP1576644A1 (fr) * 2002-12-18 2005-09-21 Koninklijke Philips Electronics N.V. Matiere piege de contaminant sur une couche de fond reflechissant aux uv dans des lampes fluorescentes
US7472576B1 (en) 2004-11-17 2009-01-06 State Of Oregon Acting By And Through The State Board Of Higher Education On Behalf Of Portland State University Nanometrology device standards for scanning probe microscopes and processes for their fabrication and use
JP2006351460A (ja) * 2005-06-20 2006-12-28 Matsushita Electric Ind Co Ltd 冷陰極蛍光ランプおよびバックライトユニット
JP4109314B2 (ja) * 2005-05-31 2008-07-02 松下電器産業株式会社 外部電極型蛍光ランプ、バックライトユニット及び液晶テレビ
WO2007004464A1 (fr) * 2005-07-06 2007-01-11 Matsushita Electric Industrial Co., Ltd. Lampe à décharge, unité de rétroéclairage, et affichage à cristaux liquides
US8040061B2 (en) * 2007-09-07 2011-10-18 Osram Sylvania Inc. Ceramic discharge vessel having an opaque zone and method of making same
CN102592944A (zh) * 2011-01-06 2012-07-18 光晔科技股份有限公司 紫外线冷阴极荧光灯

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US4684847A (en) * 1983-12-20 1987-08-04 U.S. Philips Corporation Glass composition suitable for use in a fluorescent lamp, tube and lamp envelope manufactured from said glass composition, and fluorescent lamp having a lamp envelope manufactured from said glass composition
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US7591279B2 (en) 2001-08-24 2009-09-22 Cummins Filtration Ip Inc. Controlled release of additives in fluid systems
US8109287B2 (en) 2001-08-24 2012-02-07 Cummins Filtration Ip, Inc. Controlled release of additives in fluid systems
US20060271132A1 (en) * 2003-05-24 2006-11-30 Ledeep Llc Skin tanning and light therapy system and method
US7819910B2 (en) * 2003-05-24 2010-10-26 Ledeep Llc Skin tanning and light therapy system
US20050182461A1 (en) * 2003-12-09 2005-08-18 Medx Health Corp. Shape-adaptable and spectral-selective distributed light sources using passive host medium
US7878203B2 (en) * 2003-12-09 2011-02-01 Medx Health Corp. Phototherapeutic treatment method using a passive host medium containing nanoparticles
US7921853B2 (en) 2004-03-09 2011-04-12 Ledeep Llc Phototherapy method for treating psoriasis
US20080039907A1 (en) * 2004-04-12 2008-02-14 Ledeep, Llc Phototherapy Systems and Methods
US8425772B2 (en) 2006-12-12 2013-04-23 Cummins Filtration Ip, Inc. Filtration device with releasable additive
US20090230837A1 (en) * 2008-03-13 2009-09-17 General Electric Company Fluorescent lamps having desirable mercury consumption and lumen run-up times
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WO2003105184A3 (fr) 2004-03-18
WO2003105184A2 (fr) 2003-12-18
EP1514293A2 (fr) 2005-03-16
AU2003241091A1 (en) 2003-12-22
CN1659681A (zh) 2005-08-24
US20050206320A1 (en) 2005-09-22
CN100377287C (zh) 2008-03-26
JP2005529461A (ja) 2005-09-29

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